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The name originally belonged to a fabric and novelty shop at nearby 23 Rue de Buci. The shop sold silk lingerie and took its name from a popular play of the moment (1800s) entitled Les Deux Magots de la Chine. Its two statues represent Chinese "mandarins," or "magicians" (and "alchemists," depending upon one's philosophical point of view), who gaze serenely over the room. These two oriental gentlemen are the source of the name for one of the great cultural landmark cafes of Saint-Germain des Pres. "Magot" literally means "stocky figurine from the Far East."[3] In 1873, the business moved to its current location in the Place Saint-Germain-des-Prés. In 1884, the business changed to a café and liquoriste, keeping the name.

Auguste Boulay bought the business in 1914, when it was on the brink of bankruptcy, for 400,000 francs (anciens). The present manager, Catherine Mathivat, is his great-great-granddaughter.

Les Deux Magots appears in The Chariot Makers (by Steve Matchett), in which the author describes Les Deux Magots as: "the first café in the quarter to be blessed by the morning sun. Its clientele pay a healthy premium for drinking there, it’s only fitting they should be the first to catch the warmth of the new day."

The café figures prominently in Abha Dawesar's novel That Summer in Paris (2006)

The café is referenced in the 1955 novel Lolita by Vladimir Nabokov. The narrator claims, "I sat with uranists in the Deux Magots."

In the 2009 novel El hombre que amaba a los perros (The Man who Loved Dogs) by Leonardo Padura it is one of the places where Trotsky's assassin, Ramon Mercader, spends time while waiting to be sent to Mexico to complete his assignment.

The café features prominently in Marco Missiroli's Atti osceni in luogo privato book about the young life of Libero Marsell, whose father will be a patron of the cafè and will befriend writer Albert Camus before the author's death.

The café is mentioned in Jean Rhys's 1938 novel, Good Morning, Midnight.